Direct imaging and chemical identification of all the atoms in a material with unknown three-dimensional structure would constitute a very powerful general analysis tool. Transmission electron microscopy should in principle be able to fulfil this role, as many scientists including Feynman realized early on1. It images matter with electrons that scatter strongly from individual atoms and whose wavelengths are about 50 times smaller than an atom. Recently the technique has advanced greatly owing to the introduction of aberration-corrected optics2,3,4,5,6,7,8. However, neither electron microscopy nor any other experimental technique has yet been able to resolve and identify all the atoms in a non-periodic material consisting of several atomic species. Here we show that annular dark-field imaging in an aberration-corrected scanning transmission electron microscope optimized for low voltage operation can resolve and identify the chemical type of every atom in monolayer hexagonal boron nitride that contains substitutional defects. Three types of atomic substitutions were found and identified: carbon substituting for boron, carbon substituting for nitrogen, and oxygen substituting for nitrogen. The substitutions caused in-plane distortions in the boron nitride monolayer of about 0.1 Å magnitude, which were directly resolved, and verified by density functional theory calculations. The results demonstrate that atom-by-atom structural and chemical analysis of all radiation-damage-resistant atoms present in, and on top of, ultra-thin sheets has now become possible.
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We thank L. M. Brown, J. N. Coleman, P. Rez and J. C. H. Spence for discussions. Research at Oak Ridge National Laboratory (M.F.C., T.J.P., M.P.O., S.T.P. and S.J.P.) was sponsored by the Division of Materials Sciences and Engineering of the US Department of Energy. Research at Vanderbilt was supported in part by the US Department of Energy grant DE-FG02- 09ER46554 and the McMinn Endowment. Computations were performed at the National Energy Research Scientific Computing Center at Lawrence Berkeley National Laboratory.
Author Contributions O.L.K. initiated the project and wrote the paper, M.F.C., N.D., O.L.K. and M.F.M. recorded preliminary experimental data, M.F.C. improved the imaging and recorded the data used in the paper, V.N. prepared the samples, O.L.K. and N.D. performed data processing and analysis, T.J.P. and S.T.P. performed DFT calculations, M.P.O. performed image calculations, S.J.P. initiated the aberration-corrected microscopy project at ORNL and advised on the paper, and G.J.C., N.D., O.L.K., M.F.M, C.S.O. and Z.S.S. designed and built the electron microscope. All the authors read and commented on the manuscript.
This file contains Supplementary Methods and Materials, Supplementary References and Supplementary Figures S1-S3 with legends.
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Scientific Reports (2018)